Two types of advanced nano-composite materials have been formed by incorporating as-synthesized wet-state zeolitic imidazolate frameworks-8 (ZIF-8) nano-particles into a polybenzimidazole (PBI) polymer. The loadings of ZIF-8 particles in the two membranes (i.e., 30/70 (w/w) ZIF-8/PBI and 60/40 (w/w) ZIF-8/PBI) are 38.2 vol % and 63.6 vol %, respectively. Due to different ZIF-8 loadings, variations in particle dispersion, membrane morphology and gas separation properties are observed. Gas permeation results suggest that intercalation occurs when the ZIF-8 loading reaches 63.6 vol %. The incorporation of ZIF-8 particles significantly enhances both solubility and diffusion coefficients but the enhancement in diffusion coefficient is much greater. Mixed gas tests for H-2/CO2 separation were conducted from 35 to 230 degrees C, and both membranes exhibit remarkably high H-2 permeability and H-2/CO2 selectivity. The 30/70 (w/w) ZIF-8/PBI membrane has an H-2/CO2 selectivity of 26.3 with an H-2 permeability of 470.5 Barrer, while the 60/40 (w/w) ZIF-8/PBI membrane has an H-2/CO2 selectivity of 12.3 with an H-2 permeability of 2014.8 Barrer. Mixed gas data show that the presence of CO or water vapor impurity in the feed gas stream does not significantly influence the membrane performance at 230 degrees C. Thus, the newly developed H-2-selective membranes may have bright prospects for hydrogen purification and CO2 capture in realistic industrial applications such as syngas processing, integrated gasification combined cycle (IGCC) power plant and hydrogen recovery. Copyright (c) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.